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The performance of carbon fiber (CF)–reinforced thermoplastic composites is influenced by the interfacial adhesion strength of the fiber and thermoplastic matrix. In this study, the electrophoretic coating of silane-grafted polyphenylene sulfide (PPS) particles on the CF surface was used to quantitatively control the interfacial adhesion between the CF and PPS matrix. The mechanism of the modification method was discussed, and the interfacial shear strength of the CF/PPS composites was numerically and experimentally investigated and found to be significantly higher (65.8 ± 4.76 MPa) than that of conventional thermoplastic systems. Scanning electron and atomic force microscopies of the fractured surfaces confirmed that the predominant failure mechanisms involved the deformation and breakage of the matrix due to the strong interphase in the interfacial region. A straightforward and controllable electrophoretic …